Sediment sources and sealed-pavement area drive polycyclic aromatic hydrocarbon and metal occurrence in urban streams

Metals and polycyclic aromatic hydrocarbons (PAHs) are common pollutants in urban streambed sediment, yet their occurrence is highly variable and difficult to predict. To investigate sources of PAHs and metals to streambed sediment, we sampled pavement dust, soil, and streambed sediment in 10 urban watersheds in three regions of the United States and applied a fallout-radionuclide-based sediment-source analysis to quantify the pavement dust contribution to stream sediment (%dust). We also mapped the area of sealcoated pavement in each watershed (%sealed) to investigate the role of coal-tar pavement sealant (CTS) as a PAH source. Median total and carbon-normalized total PAH concentrations were significantly higher in streambed sediment in the Northeast (54.3 mg/kg and 2.71 mg/gOC) and Southeast (5.37 mg/kg and 1.36 mg/gOC), where CTS is commonly used, than in the Northwest (2.11 mg/kg and 0.071 mg/gOC), where CTS is rarely used. Generalized additive models indicated that %sealed and in some cases %dust significantly affected total PAH concentrations in streambed sediments. The %dust was a significant variable for common urban metals: Cu, Pb, and Zn. These findings advance our quantitative understanding of the role of pavement dust as a source and a vector of contaminants to urban streams.